ALBERT

Description: Space-borne observation of methane from atmospheric infrared sounder version 6: validation and implications for data analysis Atmospheric Measurement Techniques Discussions, 8, 8563-8597, 2015 Author(s): X. Xiong, F. Weng, Q. Liu, and E. Olsen Atmospheric Methane (CH 4 ) is generated as a standard product in recent version of the hyperspectral Atmospheric Infrared Sounder (AIRS-V6) aboard NASA's Aqua satellite at the NASA Goddard Earth Sciences Data and Information Services Center (NASA/GES/DISC). Significant improvements in AIRS-V6 was expected but without a thorough validation. This paper first introduced the improvements of CH 4 retrieval in AIRS-V6 and some characterizations, then presented the results of validation using ~ 1000 aircraft profiles from several campaigns spread over a couple of years and in different regions. It was found the mean biases of AIRS CH 4 at layers 343–441 and 441–575 hPa are −0.76 and −0.05 % and the RMS errors are 1.56 and 1.16 %, respectively. Further analysis demonstrates that the errors in the spring and in the high northern latitudes are larger than in other seasons or regions. The error is correlated with Degree of Freedoms (DOFs), particularly in the tropics or in the summer, and cloud amount, suggesting that the "observed" spatiotemporal variation of CH 4 by AIRS is imbedded with some artificial impact from the retrieval sensitivity in addition to its variation in reality, so the variation of information content in the retrievals needs to be taken into account in data analysis of the retrieval products. Some additional filtering (i.e. rejection of profiles with obvious oscillation as well as those deviating greatly from the norm) for quality control is recommended for the users to better utilize AIRS-V6 CH 4 , and their implementation in the future versions of the AIRS retrieval algorithm is under consideration.

Description: Impact of aerosols on the OMI tropospheric NO 2 retrievals over industrialized regions: how accurate is the aerosol correction of cloud-free scenes via a simple cloud model? Atmospheric Measurement Techniques Discussions, 8, 8385-8437, 2015 Author(s): J. Chimot, T. Vlemmix, J. P. Veefkind, J. F. de Haan, and P. F. Levelt The Ozone Monitoring Instrument (OMI) instrument has provided daily global measurements of tropospheric NO 2 for more than a decade. Numerous studies have drawn attention to the complexities related to measurements of tropospheric NO 2 in the presence of aerosols. Fine particles affect the OMI spectral measurements and the length of the average light path followed by the photons. However, they are not explicitly taken into account in the current OMI tropospheric NO 2 retrieval chain. Instead, the operational OMI O 2 -O 2 cloud retrieval algorithm is applied both to cloudy scenes and to cloud free scenes with aerosols present. This paper describes in detail the complex interplay between the spectral effects of aerosols, the OMI O 2 -O 2 cloud retrieval algorithm and the impact on the accuracy of the tropospheric NO 2 retrievals through the computed Air Mass Factor (AMF) over cloud-free scenes. Collocated OMI NO 2 and MODIS Aqua aerosol products are analysed over East China, in industrialized area. In addition, aerosol effects on the tropospheric NO 2 AMF and the retrieval of OMI cloud parameters are simulated. Both the observation-based and the simulation-based approach demonstrate that the retrieved cloud fraction linearly increases with increasing Aerosol Optical Thickness (AOT), but the magnitude of this increase depends on the aerosol properties and surface albedo. This increase is induced by the additional scattering effects of aerosols which enhance the scene brightness. The decreasing effective cloud pressure with increasing AOT represents primarily the absorbing effects of aerosols. The study cases show that the actual aerosol correction based on the implemented OMI cloud model results in biases between −20 and −40 % for the DOMINO tropospheric NO 2 product in cases of high aerosol pollution (AOT ≥ 0.6) and elevated particles. On the contrary, when aerosols are relatively close to the surface or mixed with NO 2 , aerosol correction based on the cloud model results in overestimation of the DOMINO tropospheric NO 2 product, between 10 and 20 %. These numbers are in line with comparison studies between ground-based and OMI tropospheric NO 2 measurements under conditions with high aerosol pollution and elevated particles. This highlights the need to implement an improved aerosol correction in the computation of tropospheric NO 2 AMFs.

Description: Sensitivity of thermal infrared sounders to the chemical and micro-physical properties of UTLS secondary sulphate aerosols Atmospheric Measurement Techniques Discussions, 8, 8439-8481, 2015 Author(s): P. Sellitto and B. Legras Monitoring upper tropospheric-lower stratospheric (UTLS) secondary sulphate aerosols and their chemical and micro-physical properties from satellite nadir observations is crucial to better understand their formation and evolution processes and then to estimate their impact to the UTLS chemistry, and on regional and global radiative balance. Here we present a study aimed at the evaluation of the sensitivity of thermal infrared (TIR) satellite nadir observations to the chemical composition and the size distribution of idealized UTLS sulphate aerosol layers. The extinction properties of sulphuric acid/water droplets, for different sulphuric acid mixing ratios and temperatures, are systematically analysed. The extinction coefficients are derived by means of a Mie code, using refractive indexes taken from the GEISA (Gestion et Étude des Informations Spectroscopiques Atmosphériques: Management and Study of Spectroscopic Information) spectroscopic database and log-normal size distributions with different effective radii and number concentrations. IASI (Infrared Atmospheric Sounding Interferometer) pseudo-observations are generated using forward radiative transfer calculations performed with the 4A (Automatized Atmospheric Absorption Atlas) radiative transfer model, to estimate the impact of the extinction of idealized aerosol layers, at typical UTLS conditions, on the brightness temperature spectra observed by this satellite instrument. We found a marked and typical spectral signature of these aerosol layers between 700 and 1200 cm −1 , due to the absorption bands of the sulphate and bi-sulphate ions and the undissociated sulphuric acid, with the main absorption peaks at 1170 and 905 cm −1 . The dependence of the aerosol spectral signature to the sulphuric acid mixing ratio, and effective number concentration and radius, as well as the role of interferring parameters like the ozone, sulphur dioxide, carbon dioxide and ash absorption, and temperature and water vapour profile uncertainties, are analyzed and critically discussed.

Description: Global cloud top height retrieval using SCIAMACHY limb spectra: model studies and first results Atmospheric Measurement Techniques Discussions, 8, 8295-8352, 2015 Author(s): K.-U. Eichmann, L. Lelli, C. von Savigny, H. Sembhi, and J. P. Burrows Cloud top heights (CTH) were retrieved for the period 1 January 2003 to 7 April 2012 using height-resolved limb spectra measured with the Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) on board ENVISAT (ENVIronmental SATellite). In this study, we tested the sensitivity of the colour index method used in the retrieval code SCODA (SCIAMACHY Cloud Detection Algorithm) and the accuracy of the retrieved CTHs in comparison to other methods. Sensitivity studies using the radiative transfer model SCIATRAN showed that the method is capable of generally detecting cloud tops down to about 5 km and very thin cirrus clouds even up to the tropopause. Volcanic particles can also be detected that occasionally reach the lower stratosphere. Low clouds at 2–3 km can only be retrieved under very clean atmospheric conditions, as light scattering of aerosols interferes with the cloud retrieval. Upper tropospheric ice clouds are detectable for cloud optical depths down to about τ N = 0.005, which is in the subvisual range. The detection sensitivity decreases towards the surface. An optical thickness of roughly 0.1 was the lower detection limit for water cloud top heights at 5 km. This value is much lower than thresholds reported for the passive cloud detection in nadir viewing direction. Comparisons with SCIAMACHY nadir cloud top heights, calculated with the Semi-Analytical CloUd Retrieval Algorithm (SACURA), showed a good agreement in the global cloud field distribution. But only opaque clouds (τ N 〉 5) are detectable with the nadir passive retrieval technique in the UV-visible and infrared wavelength range. So due to the frequent occurrence of thin and sub-visual cirrus clouds in the tropics, large cloud top height deviations were detected between both viewing geometries. Also the land/sea contrast seen in nadir retrievals was not detected in limb mode. Co-located cloud top height measurements of the limb viewing Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on ENVISAT for the period from January 2008 to March 2012 were compared, showing good agreement to within 1 km, which is smaller than the vertical field of view of both instruments. Lower stratospheric aerosols from volcanic eruptions occasionally interfered with the cloud retrieval and inhibited detection of tropospheric clouds. Examples of the impact of these events are shown for the volcanoes Kasatochi in August 2008, Sarychev Peak in June 2009, and Nabro in June 2010. Long-lasting aerosol layers were detected after these events in the Northern Hemisphere down to the tropics. Particle top heights up to about 22 km were retrieved in 2009, when the enhanced lower stratospheric aerosol layer persisted for about 7 months. Up to about 82 % of the Northern hemispheric lower stratosphere between 30° and 70° was covered by scattering particles in August 2009 and nearly half in October 2008.

Description: Operation of the Airmodus A11 nano Condensation Nucleus Counter at various inlet pressures, various operation temperatures and design of a new inlet system Atmospheric Measurement Techniques Discussions, 8, 8483-8508, 2015 Author(s): J. Kangasluoma, A. Franchin, J. Duplissy, L. Ahonen, F. Korhonen, M. Attoui, J. Mikkilä, K. Lehtipalo, J. Vanhanen, M. Kulmala, and T. Petäjä Measuring sub-3 nm particles outside of controlled laboratory conditions is a challenging task, as many of the instruments are operated at their limits and are subjected to changing ambient conditions. In this study, we advance the current understanding on the operation of Airmodus A11 nano Condensation Nucleus Counter (nCNC), which consists of a A10 Particle Size Magnifier (PSM) and A20 condensation particle counter (CPC). We explore the effect of the inlet line pressure on the measured particle concentration. We identify two different regions inside the instrument where supersaturation of working fluid can take place. We show the possibility of varying the cut-off of the instrument from 1 to 6 nm, a wider size range than the one usually covered by the PSM. We also present a new inlet system, which allows automated measurements of the background, minimizes the diffusion losses in the sampling line and is equipped with an electrostatic filter to remove ions. Finally, our view of the guidelines for optimal use of the Airmodus nCNC are provided.

Description: Known and unknown unknowns: the application of ensemble techniques to uncertainty estimation in satellite remote sensing data Atmospheric Measurement Techniques Discussions, 8, 8509-8562, 2015 Author(s): A. C. Povey and R. G. Grainger This paper discusses a best-practice representation of uncertainty in satellite remote sensing data. An estimate of uncertainty is necessary to make appropriate use of the information conveyed by a measurement. Traditional error propagation quantifies the uncertainty in a measurement due to well-understood perturbations in a measurement and auxiliary data – known, quantified "unknowns". The underconstrained nature of most satellite remote sensing observations requires the use of various approximations and assumptions that produce non-linear systematic errors that are not readily assessed – known, unquantifiable "unknowns". Additional errors result from the inability to resolve all scales of variation in the measured quantity – unknown "unknowns". The latter two categories of error are dominant in underconstrained remote sensing retrievals and the difficulty of their quantification limits the utility of existing uncertainty estimates, degrading confidence in such data. This paper proposes the use of ensemble techniques to present multiple self-consistent realisations of a data set as a means of depicting unquantified uncertainties. These are generated using various systems (different algorithms or forward models) believed to be appropriate to the conditions observed. Benefiting from the experience of the climate modelling community, an ensemble provides a user with a more complete representation of the uncertainty as understood by the data producer and greater freedom to consider different realisations of the data.

Description: Improved stratospheric aerosol extinction profiles from SCIAMACHY: validation and sample results Atmospheric Measurement Techniques Discussions, 8, 8353-8383, 2015 Author(s): C. von Savigny, F. Ernst, A. Rozanov, R. Hommel, K.-U. Eichmann, V. Rozanov, J. P. Burrows, and L. W. Thomason Stratospheric aerosol extinction profiles have been retrieved from SCIAMACHY/Envisat measurements of limb-scattered solar radiation. The retrieval is an improved version of an algorithm presented earlier. The retrieved aerosol extinction profiles are compared to co-located aerosol profile measurements with the SAGE II solar occultation instrument at a wavelength of 525 nm. Comparisons were carried out with two versions of the SAGE II data set (version 6.2 and the new version 7.0). In a global average sense the SCIAMACHY and the SAGE II version 7.0 extinction profiles agree to within about 10 % for altitudes above 15 km. Larger relative differences (up to 40 %) are observed at specific latitudes and altitudes. We also find differences between the two SAGE II data versions of up to 40 % for specific latitudes and altitudes. Sample results on the latitudinal and temporal variability of stratospheric aerosol extinction and optical depth during the SCIAMACHY mission period are presented. The results indicate that a series of volcanic eruptions is responsible for the increase in stratospheric aerosol optical depth from 2002 to 2012. Above about 28 km altitude volcanic eruptions are found to have negligible impact in the period 2002 to 2012.

Description: Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry Atmospheric Measurement Techniques Discussions, 8, 8599-8644, 2015 Author(s): K. R. Daellenbach, C. Bozzetti, A. Křepelová, F. Canonaco, R. Wolf, P. Zotter, P. Fermo, M. Crippa, J. G. Slowik, Y. Sosedova, Y. Zhang, R.-J. Huang, L. Poulain, S. Szidat, U. Baltensperger, A. S. H. Prévôt, and I. El Haddad Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make impractical its deployment at sufficient sites to determine regional characteristics. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM 1 , PM 2.5 , PM 10 ) collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g. AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60–91 %) achieved using this technique, together with low detection limits (0.8 μg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon, oxygen containing and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g. filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially-resolved long-term datasets.

Description: Metrology of ground-based satellite validation: co-location mismatch and smoothing issues of total ozone comparisons Atmospheric Measurement Techniques Discussions, 8, 8023-8082, 2015 Author(s): T. Verhoelst, J. Granville, F. Hendrick, U. Köhler, C. Lerot, J.-P. Pommereau, A. Redondas, M. Van Roozendael, and J.-C. Lambert Comparisons with ground-based correlative measurements constitute a key component in the validation of satellite data on atmospheric composition. The error budget of these comparisons contains not only the measurement uncertainties but also several terms related to differences in sampling and smoothing of the inhomogeneous and variable atmospheric field. A versatile system for Observing System Simulation Experiments (OSSEs), named OSSSMOSE, is used here to quantify these terms. Based on the application of pragmatic observation operators onto high-resolution atmospheric fields, it allows a simulation of each individual measurement, and consequently also of the differences to be expected from spatial and temporal field variations between both measurements making up a comparison pair. As a topical case study, the system is used to evaluate the error budget of total ozone column (TOC) comparisons between on the one hand GOME-type direct fitting (GODFITv3) satellite retrievals from GOME/ERS2, SCIAMACHY/Envisat, and GOME-2/MetOp-A, and on the other hand direct-sun and zenith-sky reference measurements such as from Dobsons, Brewers, and zenith scattered light (ZSL-)DOAS instruments respectively. In particular, the focus is placed on the GODFITv3 reprocessed GOME-2A data record vs. the ground-based instruments contributing to the Network for the Detection of Atmospheric Composition Change (NDACC). The simulations are found to reproduce the actual measurements almost to within the measurement uncertainties, confirming that the OSSE approach and its technical implementation are appropriate. This work reveals that many features of the comparison spread and median difference can be understood as due to metrological differences, even when using strict co-location criteria. In particular, sampling difference errors exceed measurement uncertainties regularly at most mid- and high-latitude stations, with values up to 10 % and more in extreme cases. Smoothing difference errors only play a role in the comparisons with ZSL-DOAS instruments at high latitudes, especially in the presence of a polar vortex. At tropical latitudes, where TOC variability is lower, both types of errors remain below about 1 % and consequently do not contribute significantly to the comparison error budget. The detailed analysis of the comparison results, including now the metrological errors, suggests that the published random measurement uncertainties for GODFITv3 reprocessed satellite data are potentially overestimated, and adjustments are proposed here. This successful application of the OSSSMOSE sytem to close for the first time the error budget of TOC comparisons, bodes well for potential future applications, which are briefly touched upon.

Description: Gas adsorption and desorption effects on cylinders and their importance for long-term gas records Atmospheric Measurement Techniques Discussions, 8, 8083-8112, 2015 Author(s): M. C. Leuenberger, M. F. Schibig, and P. Nyfeler It is well known that gases adsorb on many surfaces, in particular metal surfaces. There are two main forms responsible for these effects (i) physisorption and (ii) chemisorption. Physisorption is associated with lower binding energies in the order of 1–10 kJ mol −1 compared to chemisorption ranging from 100 to 1000 kJ mol −1 . Furthermore, chemisorption forms only monolayers, contrasting physisorption that can form multilayer adsorption. The reverse process is called desorption and follows similar mathematical laws, however, it can be influenced by hysteresis effects. In the present experiment we investigated the adsorption/desorption phenomena on three steel and three aluminium cylinders containing compressed air in our laboratory and under controlled conditions in a climate chamber, respectively. We proved the pressure effect on physisorption for CO 2 , CH 4 and H 2 O by decanting one steel and two aluminium cylinders completely. The CO 2 results for both cylinders are in excellent agreement with the pressure dependence of a monolayer adsorption model. However, adsorption on aluminium ( 〈 0.05 and 0 ppm for CO 2 and H 2 O) was about 10 times less than on steel ( 〈 0.41 ppm and about 〈 2.5 ppm, respectively). The CO 2 amounts adsorbed (5.8 × 10 19 CO 2 molecules) corresponds to about the five-fold monolayer adsorption indicating that the effective surface exposed for adsorption is significantly larger than the geometric surface area. Adsorption/desorption effects were minimal for CH 4 and for CO. However, the latter dependence requires further attention since it was only studied on one aluminium cylinder with a very low mole fraction. In the climate chamber the cylinders were exposed to temperatures between −10 and +50 °C to determine the corresponding temperature coefficients of adsorption. Again, we found distinctly different values for CO 2 ranging from 0.0014 to 0.0184 ppm °C −1 for steel cylinders and −0.0002 to −0.0003 ppm °C −1 for aluminium cylinders. The reversed temperature dependence for aluminium cylinders point to significantly lower desorption energies than for steel cylinders and might at least partly be due to temperature and gas consumption induced pressure changes. Temperature coefficients for CH 4 , CO and H 2 O adsorption were, within their error bands, insignificant. These results do indicate the need for careful selection and usage of gas cylinders for high precision calibration purposes such as requested in trace gas applications.